Method of and apparatus for effecting the electrochemical transformation of materialin the presence of antenna electrodes



Aprll 26, 1949. w. J. COTTON 2,468,177

METHOD OF AND APPARATUS FOR EFFECTING THE ELECTROCHEMICAL TRANSFORMATIONOF MATERIAL IN THE PRESENCE OF ANTENNA ELECTRODES 3 Sheets-Sheet 1 FiledAug. 17, 1943 & l 37 3g flat/afar I F 4y v A i 1 g 1 'j z; i v j z 22 ifI M f #229 2.4! 324 W v x 1 MIL Z m: i"? .6/ 2527 2 {4 if.

2,468,1 77 THE ELECTROCHEMICAL ENCE April 1949- w. J. COTTON METHOD OFAND APPARATUS FOR EFFECTING TRANSFORMATION OF MATERIAL IN THE PRES 0FANTENNA ELECTRODES 3 Sheets-Sheet 2 Filed Aug. 17, 1943 0 5 Q I A 4 553; afia a 0 ww w w A ril 26, 1949- w. J. COTTON METHOD OF AND APPARATUSFOR EFFECTING THE ELECTROCHEMICAL TRANSFORMATION OF MATERIAL IN THEPRESENCE OF ANTENNA ELECTRODES Filed Aug. 1'7, 1943 3 Sheets-Sheet 3 1g.5 4% f I V /49' J7 1; A? /4Z a? y M E 5% h 7 @7 I V /1?/ L "/fiZPatented Apr. 1949 UNITED STATES METHOD OF AND APPARATUS FOR EFFECT- INGTHE ELECTROCHEMICAL TRANSFOR- MATION F MATERIAL IN THE PRESENCE OFANTENNA ELECTRODES William J. Cotton, Chicora, Pa, assignor, by mesneassignments, to Koppers Company, Inc, a corporation of DelawareApplication August 17, 1943, Serial No. 498,999

the starting material being effected with an increase of chemicalefliciency, production capacity of the reactor and the electricalenergytransfer emciency from the source of energy to the reactor.

In accordance with the present invention, the production capacity of areactor having a single pair of high frequency electrodes, comprising ahot electrode and its corresponding antenna electrodes may betremendously increased by increasing the number of pairs of highfrequency electrodes.

The invention is also directed to improvements wherein the electricalenergy supplied to the hot electrode, herein referred to as the "primaryelectrode," is distributed over a plurality of electrode terminals tothereby increase the working life of the reactor and to simultaneouslyincrease the chemical eiliciency of the reactor.

It is therefore the principal object of the present invention to providean improved method and an improved apparatus whereby electrical energymay be transferred from a source of cyclic electrical energy to areactor and the discharge zone therein with relatively little loss ofelectrical energy. More specifically, it is an object of the presentinvention substantially to increase the electrical energy transferefficiency of the apparatus herein set forth. It is a further object ofthe present invention to provide an apparatus for the electrochemicaltransformation of gaseous material which efiects an increase in chemicalemciency and the production capacityof the reactor.

The present invention, in one form, is directed to an electrochemicalapparatus for effecting the electrochemical transformation or gaseousmaterial. The apparatus comprises a source of cyclic electrical energy,which may be high frequency energy of the character herein set forth,and a reactor, said reactor comprising means to introduce reactingmaterial and means to removereaction products therefrom.

The reactor is provided with a hot electrode, which is connected to thesource of electrical energy, said electrode being herein designated, forpurposes of convenience of description, as the primary electrode. Theprimary electrode is provided with a pluralitysof electrode terminalsdistributing electrical energy supplied to said primary electrode tothereby increase the working life of the reactor and simultaneouslyincrease 2 the chemical efficiency of the reactor. The reactor isprovided with a plurality of secondary reactor-electrode terminalscooperating with the primary electrode terminals, and. means are alsoprovided to increase the energy transfer from said source of cyclicenergy to the reactor to above about 60%; and usually this increase inenergy transfer may be as much as 80% to 85%, or even greater. By theexpression means to increase the energy transfer from the source ofcyclic energy to the reactor is meant such means as will produce at thereactor discharge a certain percentage of the cyclic energy produced-bythe generator.

While it is desirable to increase the energy transfer from the source ofcyclic energy to the reactor to at least 80%, the invention in its broadaspect is not limited to an increase of this character, and theprinciples of the invention may be employed with a much lower increasein electrical energy transfer efficiency.

In one form of the present invention, the primary reactor electrodeterminals which are connected to a source of cyclic energy, as, forexample, high frequency energy of the character herein set forth,cooperate with a plurality of secondary reactor electrode terminals,each of which are separately connected to a separate antenna in circuitwith said source of cyclic electrical energy to thereby insure thetransfer of electrical energy from the source of said energy to thereactor with relatively low transfer loss. In one form of the invention,each antenna is conditioned to cause the initiation of a plurality ofdischarges in said reactor on the passage of cyclic energy, as, forexample, high frequency energy of radio or radar frequency, or muchlower, through the hot or primary electrode. In another form of theinvention, although separate discharges are initiated,

these discharges merge together with discharges produced by a crosseddischarge to form a single composite discharge volume.

In accordance with the present invention, a reactor of the characterabove set forth may also have present a separate set of cooperatingelecminals.

The advantages resultin from the use of crossed discharges is set forthin copending application Serial No. 546,882, filed July 27, 194A,Electrochemical transformation of gaseous material, acontinuation-in-part of application Serial No. 483,931, now abandoned.It is desired to point out that all the advantages resulting from theuse of crossed discharges are also obtained when utilizing the methodand apparatus herein set forth, whereby not only is there an increase inchemical yield produced by the crossing of the discharges, butsimultaneously with this increase in chemical yield there is obtained anincrease of production capacity, as hereinafter more fully pointed out.

Further. in the preferred form of the invention, when using crosseddischarges, the cyclic energy supplied to the hot electrode isdistributed to a plurality of electrode terminals to thereby increasethe working life of the reactor, and in this manner simultaneouslyincrease the chemical efiiciency of the reactor.

In one form of the invention, the antennas are coupled to inductances,said inductances being of a character to provide the initiation of Whatmay be termed a relatively fat discharge. Other equivalent means may beused to tune the antennas so that the circuit of which said antennas area part will assist in producing a desirable full volume discharge in thereactor on the passage of cyclic energy through the reactor electrodes,either in the presence or without the presence of crossed dischargesgenerated by a separate set of cooperating crossed electrodes.

The reactor herein set forth, in the preferred form of the invention, isin combination with a generator unit including a tank circuit connectingthe generator unit to the reactor, said generator unit functioning as asource of cyclic energy. The tank circuit preferably includes aplurality of antennas, each respectively in operative connection withsaid secondary cooperating electrodes, said tank circuit being tuned tocause the initiation of a plurality of discharges, preferably fullvolume discharges, in the reactor on the passage of cyclic energythrough the hot electrode. In the preferred form of the invention, thereactor of the electrochemical apparatus is provided with a hotelectrode which is incapable of oxidation at the temperature present inthe reactor. Desirably, it has a melting point of the order of thatpossessed by tantalum, whereby oxidation of the electrode is inhibitedat the temperature present in the reactor.

While it has been stated that the primary or hot electrode terminals areof tantalum or equivalent material, it is within the province of thepresent invention to have all of the terminals present in the reactor oftantalum or equivalent material, it being pointed out that it has beendiscovered that columbium, thorium, thoriated tantalum, and thoriatedcolumbium are exceedingly valuable as electrode or electrode terminalmaterials.

It is within the province of the present inventlon to supply to the hotor primary electrode cyclic energy, which may be defined as highfrequency energy. said energy having a. periodicity varying from about10,000 cycles to about 300,000 mc. This corresponds in wave length from30,000 meters to 1 mm. or less. The present invention may be carried outby supplying a high frequency current to the hot electrode varying infrequency from about 250,000 cycles, or even 500,000 cycles, to 300,000me. or over. As a practical matter, the invention finds its greatestfield of usefulness when the electrochemical transformation of materialsis efiected using high frequency energy of the order of radio frequencyor radar frequency.

When the invention is used in a reactor gen-- erating crosseddischarges, the crossing electrodes may be supplied with low frequencyenergy, that is, energy varying from 10 cycles to 3,000 me. or more, butusually within the limits of 25 cycles to 10,000 cycles. In one form ofthe invention, the two frequencies supplied to the crossed electrodesshould differ in numerical value one from the other. The order of thedifference, in'this preferred, specific form of the invention, is thatthe crossed frequencies simultaneously acting on a chemical material andelectrochemically transforming said material, should roduce an increasein chemical yield of the final reaction product over that yield whichwould be produced using only the particular low frequency of the crosseddischarges, or in using only the particular high frequency of thecrossed discharges. However, it is to be understood that the frequencieswhich are crossed in the reactor herein referred to may be ofsubstantially equal frequencies, and highly advantageous results arethus obtained.

The present invention will be illustrated in connection with theaccompanying drawing, in which Fig. 1 is a cross-sectional view of areactor capable of generating crossed discharges of the character hereindescribed, said reactor being provided with low frequency electrodes andwith a high frequency electrode connected in the tank circuit of thegenerator, said reactor also being provided with high frequency antennaelectrodes;

Fig. 2 is a cross-sectional view taken on the line 2-2 of Fig. 1;

Fig. Bis a cross-sectional view taken on the line 33 of Fig. 1;

Fig. 4 is a cross-sectional view taken on the line 0-4 of Fig. 1;

Fig. 5 is a cross-sectional view of a reactor in which a plurality ofelectrodes is provided, oneof which is a so-called primary hot electrodedirectly connected in the tank circuit of a generator, said hotelectrode being provided with a plurality of primary electrodeterminals, the remaining electrodes functioning as ground electrodes viaantenna circuits v Fig. 6 is a cross-sectional view taken on the line6--6 of Fig. 5;

Fig. '7 is a. cross-sectional view of a modified form of reactoremploying a. high frequency primary hot electrode and a plurality ofsecondary antenna electrodes;

Fig. 8 is a diagrammatic representation of an apparatus for drying airprior to its introduction into the reactor and fur absorbing the nitricoxide content of the exit reaction gases:

Fig.9 further sets forth the hook-up of the high frequency generatorused in providing the high frequency energy supplied to the tank circuitconnecting the generator to the reactor; and

Fig. 10 sets forth the tank circuit used in conveying the electricalenergy from the generator to the reactor.

Referring to Fig. 1, the reactor unit comprises a reactor vessel Ihaving an interior wall 2, said reactor-being made of a non-conductingor insulating medium such as a ceramic material, including glass, andpreferably a highmelting point glass, as exemplified by Pyrex.

The reactor l comprises horizontally extending members orlegs 3 aud tand vertically extending members or legs 5 and 6. Positioned within thereactor leg 3 is a sheath member 1 made of glass, said sheath memberbeing mounted in an insulating closure 8. Projecting through the Isheath I is a brass electrode 9 having mounted on its interior end aseat Hi, from which extend three symmetrically arranged stud bolts ll,l2

. and I3, on the interior ends of which are screwed electrode tips l4,l5 and I6, made of any desired material, as, for example, of an alloycontaining 98% copper and 2% lithium, or equivalent materialshereinafter referred to. The electrode tips are removable, and may bereplaced at the termination of their useful life with new tips. The seatmember, stud bolts and electrodes may be made of any cheap metallicelectrical conductor, as, for example, copper or brass. Seat member l0carries ports ll, i8 and I9 extending longitudinally of the sheathmember- I to thereby provide means for the passage ofgases to thedischarge area, to there be reacted. The electrode 9 is mounted in aninsulating closure 20 and is connectedby means of a thumb screw or thelike with a lead 2|, which in turn is connected to the generator G bythe tankcircuit hereinafter set forth. Voltmeter V is included in thetanle circuit, being shown in Fig. 1, and also in Fig.10. The leg member4 is provided with an insulating end closure 22, in which is mountedsheath'member 23, the exterior end of which isprovided'with aninsulating closure 24. Projecting throughthe closure member 24 andinteriorly of the sheath member 23 are the electrodes 25, 26' and--21,made of brass or any similar material. The electrodes pass through aninsulating spacer 28', which serves to keep said electrodes electricallyseparated. Removably mounted on the'ends of said electrodes areelectrode terminals or tips 29, 30 and 3|, said electrode terminals'being made of anydesired electrode material, as, for example, of acopper lithium alloy containing 98% copper and 2% lithium. Connected tothe electrodes 25, 26 and 2'! are antennas 32, 33 and 34, which includevariable inductances 32a, 33a and 34a respectively, and

' the latter may be provided with antenna tails.

The variable inductances are used to tune each of the antenna electrodesto maximum efiiciency.

The leg 3 is provided with an inlet member 35 and leg 4 an outlet memberor conduit 36. -Positloned within the leg 5, which is preferablydiametrically opposite the leg 6, is a sheath member 31 mounted in theleg closure member 38. Passing through the leg member 5 and mounted inthe sheath end closure 39 is an electrode 48 provided with a buttonterminal member 4|, which, when hot, preferably fits snugly within thesheath member 37, said button being provided with a plurality of ports42, so as to adapt said button electrodes tobe interchanged with thehigh frequency electrodes and electrode terminals.

The electrode 43 ismounted in a sheath closure 44 of the sheath member45, said electrode being provided with a button terminal 46. The leg 6is closed by the insulating closure member 41. The button may beprovided with a plurality of 'apertures 48, said apertures serving the.same purpose as those present in button 4|.

The electrode terminals I4, l5, l6 and 29, 30,

3|, which are preferably pointed, as this increases the chemical yieldof product per kilowatt hour, may consist of any metal or alloy, such,for instance, as nickel, copper, iron, copperlithium alloy, tantalum,columbium, thorlated' tantalum, thoriated columbium, and brass. Carbonelectrodes are satisfactory under some conditions. It is broadly withinthe province of the present invention to substitute for said pointedelectrodes buttons, nodules, or globules, or to have electrode terminalsin any other shape hitherto used in the treatment or electrochemicaltransformation of chemical products.

When the electrode terminals are in the shape of sharp-pointed members,the sheath members may be omitted, but it is highly desirable to retainthem in order to force the flow'of the gaseous medium being subjected tothe action of the electrical discharge in and around the electrode tips.Further, it is desired to point out that the sheath members function, toa large extent, to protect the outer vessel from the eifect of heat,which may be produced during the course of the reac-' tion in thereactor.

It is preferred that the electrode terminals project beyond the interiorends of the sheath members in order to avoid undue heating of the sheathtubes, said avoidance of undue heating functioning to inhibit thegeneration of sodium and other undesirable ions which tend to generate.side reactions,

The diameter of each of the reactor legs is approximately 32 mm. and thediameter of the sheath members is approximately 23 mm. The overalllength of the horizontal members from the exterior end of the leg member3 to the exterior end of the leg member 4 approximates ten inches, andthe vertical members have alike overall length. These dimensions are setforth in an illustrative sense and are not to be taken primarily by wayof limitation.

While the reactor herein set forth may be used to effect theelectrochemical transformation of various materials, the operationthereof will be set forth in connection with the production of nitricoxide from atmospheric air.

The atmospheric air is dried in an apparatus of the character set forthin Fig. 8, and in the manner herein described. It is then introducedthrough the inlet member 35 into the sheath member and then passesthrough the seat member In and through the split discharge regionpresent in the reactor. The reaction product passes around the electrodeterminals 29,

30 and 3| through the sheath member 23 and leaves the reactor by meansof the exit conduit 36.

The air is dried prior to its introduction into the reactor vessel bypassing it through'the soda lime tube A, Fig. 8, then through the silicagel tube B. thence through the conduit C, through the orifice D of thedifferential manometer E, through the valve F, and thence to the reactorI. At the point H is connected the mercury manometer H1 which measuresthe internal pressure of the reactor. From the reactor I the exit gasespass through exit conduit 36 to a series of silica gel absorber tubes J,which tubes extract the nitric oxide content of the exit gases. A vacuumis applied by means of the vacuum pump K and the amount ofvacuumadjusted by means of the release valve L and the main valve? in thesupply line. The soda lime functions not only to take out a portion ofthe moisture but also to extract from the air substantially all of thecarbon dioxide. The air as delivered to the reactor has a moisturecontent of about 5 to 8 mg. of moisture per liter. When the run isstarted, the valves N and P are closed and M and 0 are open. Whenoperation has reached equilibrium, valves N and P are quickly opened andvalves M and 0 closed, noting the time of doing so with a stop-watch.

Upon conclusion of the run, valves M and O are The time interval duringwhich the valves N and P are open to the absorbers and the valves M andO of the by-pass are closed is six minutes, During this period thesilica gel is absorbing the nitric oxide produced by the reaction. Afterthe run is terminated, the silica gel tubes are weighed and the increasein weight taken as the weight of nitric oxide produced in the sixminutes.

In starting the apparatus, the flow of dried air is initiated throughthe inlet member 35, said air passing through the reactor vessel l atthe rate of approximately 500 cc. per minute, standard conditions, thepressure within the reactor vessel being maintained at approximately 335mm. mercury pressure.-

During the period that the air is passing through the reactor theelectrodes 40 and 03 are connected to a source of low frequency energy,as, for example, a source of alternating current having a frequency of60 to 500 cycles. During this interval, electrode 9 is connected to asource of high frequency energy, as, for example, 10,000 cycles to300,000 me. or over. The high frequency energy passes from the electrodeterminals I l, l5 and I6 to the electrode terminals 29, 30 and 3!through the electrodes 25, 26 and 27, and then through the antennas 32,33 and 34. The electrodes 2*, 26 and 21 .may properly be called antennaelectrodes. The high frequency current, in passing through the highfrequency electrodes and electrode terminals, tends to form distinctdischarges between the respective high frequency terminals. Thesedischarges are clearly visible closely adjacent each set of electrodeterminals but merge one into the other towards and adjacent the centerof the discharge volume. It is clear from the above that there isprovided, :in accordance with the present invention, an apparatusgenerating crossed electrical discharges, said discharges beinggenerated by low frequency electrodes which are crossed with a pluralityof high frequency electrodes, the low frequency energy and highfrequency energy being preferably, but not necessarily, of the orderherein set forth. It is desired to point out that the low frequencydischarge frequently moves about over the faces of the two buttonelectrodes.

In accordance with the present invention, the

use of a plurality of high frequency discharges greatly increases thecapacity of a'given reactor. In other words, using crossed discharges,the high frequency discharge being unsplit, and other operatingconditions remaining the same, the

capacity at maximum efiiciency of the reactor is limited to the minimumsustaining energy under which the discharge will operate, which minimumusually varies from 12 to 39 watts per pair of high frequency electrodetips, depending upon conditions, and approximatingZO Watts for the caseunder discussion.

It is desired to point out that for any pair of points the energyapplied should not exceed the minimum sustaining energy. By this ismeant that the product of the volts times the current in amperes shouldnot exceed that value which will just maintain continuous operation ofthe discharge. It must exceed the value at which the discharges flutter.Consumption of energy in excess of this amount goes primarily to heatand is thus wasted. Furthermore, the heat thus produced will partiallydecompose the products formed when using just the sustaining energy. Itis for this reason that the capacity of a reactor cannot be increased bymerely increasing the single pair of points to an efliciency which maybe as high as 90%. It is therefore clearthat the provision of a reactorin which low frequency electrodes and electrode terminals supplied withlow frequency energy are crossed with high frequency electrodes andelectrode terminals, one

of which is a hot set of electrodes and electrode terminals, and theother of which has its electrodes and electrode terminals connected toantennas, functions to significantly increase the chemical efiiciencyand production capacity of the reactor and the amount of energytransferred from the generator circuit via the tank circuit to the hotelectrode, and therefore significantly decreases power costs.

It is known in the art that by a proper balancing of the reactor load tothe generator supply the transfer efiiciency from the generator via thetank circuit to the discharge can be increased. Utilizing the apparatushereinbefore described,

- in which there are three pairs of high frequency electrodes, the loadis more nearly balanced with the generator supply, so that an increasein efflciency could normally be expected of from 1% to 2% to about 5%.However, it has been found that even when using only two pairs of highfrequency electrodes and tuning each of the am tenna electrodes tomaximum transfer efficiency. the energy transfer may be as high as 80%.This compares with the maximum efiiciency obtained in the ordinary highfrequency dielectric heating devices of between 50% and 60%.

It is desired to point out that increase of the number of pairs of highfrequency electrode terminals in one reactor increases the productioncapacity of the reactor without decreasing its chemical efficiency, 1.e., grams of product per kilowatt hour, providing each pair of terminalsis operated with no more than the sustaining energy.

More specifically, this increase in the chemical efficiency, theproduction capacity of the reactor and the transfer efiiciency, that is,the transfer of electrical energy from the generator circuit to thereactor, is accomplished by tuning each antenna by means of its variableinductance, the amount of inductance being such as to avoid theformation of a stringy discharge. By a stringy discharge is meant adischarge in which the bulk of the luminosity is concentrated along thecore. If too many or too little turns are cut in or out of the antennainductors, then the discharges may become fstringy, or weak, orfluttering, and under some circumstances may be entirely extinguished.

It is further desired to point out that adischarge of uniform luminousdensity usually coincides with a condition of maximum energy transferfrom the generator to the discharge. It is to be understood from theabove explanation that no hard and fast rule can be given for the amountof inductance which is cut in or out of each antenna 32, 33 and 3 3, butthat, functionally, it should be that amount which will insure theproduction of a uniformly luminous,

In general, this energy transfer efficiency is increased from about 1%to 2% for a mum efl'iciency of energy transfer.

non-stringy discharge, while at the same time producing a significantincrease in electrical transfer eiiiciency, which may be as much as 80%to 85%, that is, the electrical transfer efficiency is increased fromabout 1% to about 80% to 85%.

As shown in Fig. 5, there is provided a reactor which is designated asan entity by the numeral l6, said reactor having interior walls 49. Thereactor comprises horizontally extending members or legs 50 and andvertically extending leg members 52 and 53. Positioned within thereactor leg 50 is a sheath member 54 made of glass, said sheath memberbeing mounted in an insulating closure 8. Projecting through the sheath54 is an electrode 55, carrying a pointed electrode terminal tip 56. Theelectrode 55 is mounted in an insulating closure member 51, said.electrode 55 being connected to an antenna 58 in any suitable manner,as, for example, by a set screw 59. The antenna includes a variableinductance 58a and may, under some conditions, include an antenna tail58b, the latter being operatively connected to the inductance 58a. Inthe apparatus set forth in Fig. 5, it was found desirable to insert aspart of the antenna an inductance coil 58a. The capacitance'of the tankcircuit is such as not to require any additional capacitance, but doesrequire inductance in order to provide the necessary impedance, which,in turn, insures maxi- However, if the tank circuit should lacksufficient capacitance, then this may be supplied by the use of avariable condenser in lieu of or in conjunction with, either in parallelor in series, the variable inductor shown.

Positioned within the leg 5| is a similar electrode 60, having anelectrode tip or terminal 6|. The electrode 60 is mounted in the closuremember 62 which functions to close the exterior end of the sheath 63.The electrode 60 and the sheath 63 is mounted in an end closure 64 whichfunctions to close the exterior end of the leg member 5|. The electrode60 is connected to the antenna 65, which includes an inductance coil65a, and preferably a tail member 6512.

The leg member '53 is provided with an insulating end closure 66, inwhich is mounted a sheath member 61', the latter being closed at itsexterior end by an insulating closure member 68. Mounted within thelatter is an electrode member 69, provided with an electrode terminal ortip 10. The electrode 69 is connected to an antenna II, which includesan inductance Ha and preferably a tail member Mb. The leg member 52 isprovided with an insulating end closure 13, in which is mounted a sheathmember 14, the exterior end of the latter being provided with aninsulating closure 15. Mounted in the latter and passing through thesheath member 14 is an electrode 16 which is connected to a generator Gby means of a lead 11, as shown in Fig. 5 and at 2| in Fig.respectively. The generator is grounded at 18 via tank circuit; saidground being also shown in Fig. 10 at I65. The generator hook-up isshown'in Fig. 9, the generator circuit being coupled with the tankcircuit set forth in Fig. 10. The sheath member 14 is provided with aninlet member 19, and the sheath member 61 is provided with an outletmember 80.

Operatively connected to the electrode 16 is a plurality of hotelectrode terminals BI, 82 and 83, said terminals being preferablyconnected to the electrode 76 by an intermediate connection member 84,'the latter preferably being in the shape of a semi-circular discmember, and positioned within the sheath member to provide gas passages85, 86, 81 and 88 respectively of Fig. 6.

The electrodes BI, 82 and 83 are positioned in the connection member 84so as to be symmetrically arranged with respect to antenna electrodeterminals 56, I0 and 6| respectively. In the preferred form of theinvention, the electrode gap between the antenna electrode terminals andthe symmetrically placed hot electrode terminals is preferably, althoughnot necessarily, approximately equal. When the electrode terminal gapsare equal, then the tuning of the circuit is facilitated.

While the electrode terminals set forth in Fig. 5, and some of those setforth in Fig. 1, are in the shape of sharp-pointed members, it isdesired to point out that it is within the province of the presentinvention to'use buttons, nodules, globules, or to have the electrodeterminals in any other shape hitherto used in the treatment orelectrochemical transformation of chemical products. However, increasedchemical yield is obtained by using pointed electrodes. The sheathmembers set forth in the form of the apparatus shown in both Fi s. 1 and5 may be omitted, but it is highly desirable to retain them in order toforce the flow of gaseous medium being subjected to the action of theelectrical discharge'or discharges in and around the electrode tips.Further, the sheath members function to a substan tial extend to protectthe outer reactor vessel from the effect of heat which may be producedduring the course of the reaction in the reactor.

' It is preferred that the electrode terminals project beyond theinterior end of the sheath members in order to avoid undue heating,which may induce generation of sodium or other undesirable ions whichtend to generate side reactions.

By providing a plurality of electrode terminals BI, 82 and 83 instead ofa single electrode terminal, the total power of the hot electrode isdivided between a number of points rather than being concentrated all atone point. It is desired to point out that when high frequency energy issupplied to the electrode Hi, the remaining electrodes of the reactorshown in Fig. 5 being the antenna electrodes, there is produced a splitdischarge. In the form of the apparatus shown in Fig. 5, the dischargewill be triply split, the potential discharge having been split intodischarges X, Y and Z. Using the form of apparatus shown in Fig. 5, theelectrical energy transfer efiiciency from the generator through thetank circuit to the discharge is increased from approximately 1% to 2%to approximately to It is to be noted that in Fig. 5 there is provided aplurality of hot electrode terminals instead of a single electrodeterminal. This results in two advantages, namely, increased life of thehot electrode terminals 8|, 82 and 83, due to the distribution of thehigh frequency energy over three electrodes instead of beingconcentrated on one electrode; and a further advantage may be notedthatthe maximum chemical efficiency in terms of grams of product perkilowatt hour of energy supplied is at a maximum when the minimumsustaining energy, that is, the energy to sustain the discharge, whichapproximates 20 watts for the reactor shown in Fig. 5, is applied toeach pair of electrode tips between which the discharges X, Y and Z act.Since there are three hot electrode terminals-instead of one, thereactor set forth in Fig. 5 will result in a yield expressed as grams ofproduct per kilowatt hour of energy supplied, appreciably greater thanif the three hot terminals were all combined as one terminal.

It is therefore clear that the provision of a split discharge in a highfrequency reactor, the hot electrode or which is provided with aplurality of terminals and the other electrodes of which are groundelectrodes via antennas, herein designated as antenna electrodes,functions Signiflcantly to increase the amount of energy transferredfrom the generator circuit via the tank circuit to the hot electrode,and thereby significantly decrease power costs; and, further, thechemical yield and capacity is significantly increased by having aplurality of hot electrode terminals which are preferably, although notnecessarily, symmetrically positioned with regard to cooperating antennaelectrode terminals.

In Fig. 7 there is shown another form of reactor, employing a highfrequency hot electrode and a plurality of antenna electrodes. Thereactor comprises a reaction vessel or tube 09 provided with endclosures 90 and BI respectively. Mounted in the end closure 90 is asheath member 92, which is closed at its rear end by an insulatingclosure member 93. Mounted in said closure member is a plurality ofelectrode members 94, 95 and 90 provided respectively with terminalmembers st, all and 90. The electrodes 90, 95 and are carried at theirforward end by an insulating spacer member I00, which is provided withgas passages IllI. The electrodes 00, 95 and have connected theretoantennas I02. I03 and tilt, said antennas preferably includinginductances Iliila, WM and lfl la; and in most cases tails iilllb, i031)and w th are provided. Disposed in the reactor tube 0Q, diametricallyopposite sheath til, is a sheath member I05 mounted in the end closureHI. The sheath I05 is provided with an end closure I00, in which ismounted the hot electrode Hill, which seats at its forward end in a seatI 03, from which extend three symmetrically arranged stud bolts I09, H0and Ill, on the interior ends of which are screwed electrode tips Ii litand H t of any desired material, as, for example, of an alloy containing98% copper and 2% lithium, or equivalent materials, hereinafter referredto, the present invention not contemplating that any of the electrodesbe made of any specific material. The reactor is provided with an inletI I5 and an exit I It.

The electrode I0! is connected to the generator G by means of a leadII'I shown in Fig. 7 and 2I in Fig. 10. The generator is grounded at II8via tank circuit, said ground being shown in Fig. 10 at I65. Thegenerator hook-up G is shown in Fig. 9, the generator circuit beingcoupled with the tank circuit set forth in Fig. 10.

While the reactors herein disclosed may be used in the manufacture ofvarious chemical compounds, it is of particular value in the manufactureof nitric oxide from atmospheric air or air which has been enriched withoxygen. In producing nitric oxide in any of the reactors herein setforth, the air is dried in the apparatus set forth in Fig. 8, thefunction of said apparatus having been hitherto described.

In an apparatus similar to Fig. 1, using, however, only two pairs ofhigh frequency electrodes and no low frequency electrodes, the rate offlow of the air through the reactor being equal to approximately 4'70cc..per minute, standard conditions, and the pressure within the reactorbeing 730 mm. mercurcy pressure, and with a voltage at the discharge of1500 volts and 150 miniamperes per pair of points, operating under theconditions above set forth, there is obtained a transfer efliciency ofenergy transfer equal to 80.4%. It may be pointed out in this connectionthat the increase in energy transfer increased the watts per pair ofpoints from 20 to 225, and hence did not provide maximum chemicalefficiency, so that additional pairs of points are necessary to realizemaximum chemical efiiciency with transfer efficiency.

In operating reactors of the character herein set forth and equivalentreactors under a voltage of 1500 volts at the discharge and I50milliamperes per pair of points, the power of each of the discharges isgreatly in excess of the power necessary for the greatest chemicalefficiency, that is, yield expressed in grams of reacted prodnot perkilowatt hour. Having once'made this discovery, the next step was toascertain a solution of the problem whereby this excess power could beeconomically and efficiently utilized. This may be accomplished byproviding a large plurality of pairs of points. In the particularillustration set forth, two pairs of electrodes were used, each pair ofelectrodes needing only a power input at the arc of 20 watts. However,each pair of cooperating electrodes was actually supplied with 225watts, making an excess wattage for each set of electrodes of 205 watts,or a. total of the two sets of electrodes of 410 watts. Since, on anaverage, for best efliciency in electrochemical transformation, each setof electrodes requires about 20 watts, the problem was solved byproviding the reactor with 25 pairs of electrodes. In other words. thepotential discharge which will be generated by one set of electrodes issplit up into 25 discharges. These discharges usually have a separateentity at and adjacent their respective electrode terminals but begin tomerge together a short distance from the electrodes to form a continuousluminous medium.

In the above experiment, the hot electrode is supplied with highfrequency energy having a frequency of 1.91 mc. (corresponding to 157.1meters). The reactor set forth in the above experiment is one identicalwith that set forth in Fig. 5, with the exception that the electrode 60is removed from the reactor and the closure member 52 is replaced with asolid closure member. Referring to Fig. 5, used in the above experiment,the gap between the electrode terminals 56 and BI is 2'7 mm.; the gapbetween the electrode terminals 82 and I0 is 49 mm. It is desired topoint out that the antenna 58 has incorporated therein an inductance58a, the latter consisting of 438 turns of No. 28 D. C. C. wire wound ona lA-inch diameter mandrel plus an Ohmite coil known as No. 2-4. Thetail to this antenna consists of 9 feet of No. 18 copper wire.

The antennas II included an inductance Ila consisting of 454 turns ofNo. 28 D. C. C. copper wire wound on a I A-inch diameter mandrel plus anOhmite coil known as 2-3, and further included a tail of-7 /2 feet ofNo. 18 copper wire.

In the above example, the electrode terminals 50, I0 and 82 were nickel.The specific discharge gaps are set forth in an illustrative manner andnot by way of limitation, it being recognized that the discharge gapsmay vary greatly in accordance with predetermined factors, such as thevoltage under which the high frequency current is supplied, thefrequency of the high frequency energy, the pressure of the air or othergas passing through the reactor, the nature of the gas or fluid which-itis desired to electrochemically react, andsimilar factors.

-The following is an additionally illustrative example.in-i=which thereactor set forth in Fig. is

utilizecl said reactor being provided, as shown,

- with three high frequency hot electrode terminals which respectivelycooperated with three antenna electrode terminals. The frequency of theen--' e'rgy supplied'tothehot electrode 1.6 is 1191 me. (correspondingto 157.1 meters). Air is passed through-the reactor at the rate of about485 cc.

"per minute, standard conditions. and the pressure in the reactor is 337mm. of mercury. The

high frequency energyis delivered to the are undera voltage of 700 voltsand an amperage of 100 milliamperes to each of the three pairs ofelectrodes,-namely, 8I and 56; 82 and Ill; and 83 and 6|. The dischargegaps areas follows: between electrodes 8I and 56 the are gap is 33 mm.;between .electrodes 82 and 18, the discharge gap is 27 mm.; and betweenelectrode terminals 83 and 6|, the discharge gap is 16 mm. Thesedischarge gaps are deliberately varied in order to obtain results underdifferent operating conditions.

The antenna 58 has present an inductance coil 58a consisting of 438turns of No. 28 D. C. C. cop- .per wire close-wound on a lA-inchmandrel, plus an Ohmite coil No. Z-4, and further has a tail of 9 feetof No.18 copper wire. The inductance Ila of the antenna 'II consists of436 turns of No. 28 D. C. C. copperwire close-wound on a I A-inchmandrel. plus an Ohmite coil of the 2-4 type,

a plus a 10-foot tail of No. 18 copper'wire.

Theantenna 65 included an inductance 65a which consisted of 454 turns ofNo.28 D. C. C.

copper wire close-wound on a lA-inch mandrel, plusiwo. Ohmite coils,type Z-3, plus a 7 /2f00t tail .of No. 18 copper wire. 7

Inthe above experiment, the electrical transfer efiiciency is only 39%,because time was not taken ..to accurately tune each of the antennaelectrodes. When the optimum inductance is placed in each respectiveantenna, then optimum electrical transfer efficiency is obtained. Inother words, the transfer efliciency may vary from 40 to 80-85% or 90%,the latter figures representing the optimum transfer efficiency.

.It is desired to point out that the amount of inductance which eachantenna carries is such as to give what may be termed a fat discharge,that is, a discharge which is not a stringy discharge mostly core. Forexample, the arcs a X, Y and Z of Fig. 5 are maintained in a bulged-101.; state,=such as shown in Fig. 5, this being accomplished by cuttingin or out in therespective antennas induction turns.

little turns are cut in or out of the antenna,

If too many or too thn the discharge may become what is known as a"stringy or fluttering discharge. and the give optimum transferefficiencies.

Asshown in Fig. 1, the gaseous material is subjected=to a plurality ofcrossed electrical discharges,;one,,of said discharges being of the or-;der of 2 .;mc.. and the other being of the order of 560 cycles; orradio frequency energy may be crossed; with radio frequency energy, as,for exambands may be crossed with similar high frequen- 'cy having peakbands; or energy of a much lower frequency having peak bands. In all ofthese cases. the electrical transfer energy is greatly increased byproviding a plurality of pairs of electrode points with properly tunedantennas, as hereinbefore described.

' While the present invention has been set forthin connection with theproduction of nitric oxide, it may be applied to effect a number ofchemical reactions, including chemical combination, polymerization,dehydrogenation, oxidation, and the like. Organic compounds, such asaliphatic, aromatic, or cyclic hydrocarbons, aldehydes,ketones,alcohols, esters and acids, as well as nitrogen, sulphur,halogen, or other substitution products and derivatives thereof, may betreated in accordance with the principle of the present invention toeffect chemical combination, splitting or breaking down, transformationfrom saturated to unsaturated compounds, or vice versa, hydrogenation,dehydrogenation, and many other chemical reactions.

The present invention may be used for the production of aldehydes, suchas formaldehyde, for the oxidation of sulphur dioxide to sulphurtrioxide, for the condensation of ammonia to hydrazine, the oxidation ofbenzene to phenol, and the like. v

While it has been stated that the electrode terminals or tips'are madeof nickel, it iswithin the province of the present invention to employother electrode materials, such as copper, brass, tantalum, silver,iron, chomium, nickel. chromium alloys, nickel alloys, platinum alloys,columbium, thorium, and the like. Carbon electrodes may be used. Any'orall of the electrode terminals may be made of a copper lithium alloy,as, for

. example, 98% copper with 2%. lithium.

The hot electrode terminal may be made of a metal or alloy having adifferent ion emission potential from the antenna electrodes. It iswithin the province of the present invention to make the electrodes andelectrode tips of different conducting metals or alloys, so as toprovide electrode tips each chosen to have its own selective ionemission potential.

Fig. 9 sets forth the hook-up of the high frequency generator unit usedfor producing the high frequency energy'supplied to the tank circuitconnecting the generator to the reactor. The diagram may be divided intofour circuits, 'II9, I20, I2I and I22. Circuit H9 is the 'full waverectification unit wherein the leads I23 connect to the -volt 60-cyc1esupply on the panel board. The numeral I24 identifies a transformerdelivering. its secondary high voltage current to the tworectificationtubes I25, the filaments of which are heated by current generated in thefilament transformer I26. The resistor I28 and fixed condenser I29,together with the choke coil I21, constitute a filter. Thehigh voltageD. C. current produced by this circuit leaves same by means of theground connection I38 and the lead I3I, which delivers to the plate oftubes I32 and I33 of the oscillator circuit. The transformer I34,connected with a 110-volt supply, provides the filament power for thetubes I32 and I33. The desired frequency is obtained by means of ingeffected by operation of the variable condenser I35 and the inductanceI35.

In carrying out the work described as above tuning the oscillatorcircuit I28, such tuning be- 15 set forth between the limits of wavelength of 20 meters or 15 Inc. and 175 meters or 1.71 mc., it isnecessary to change the size of the inductance I36 by steps. This isdone by removing one ill-,- ductance and replacing same with anotherinductance having the desired characteristics. The minor circuit I31 isa coupling circuit, coupling the oscillator circuit I20 to the gridinput circuit I38 of the power amplifier circuit I2I. The grid circuitof the power amplifier is tuned by means of the variable condenser I39and by changing inductance coils I38 in a manner similar to the .changeeffected in inductance I36, as necessary to meet requirements. Thecombination of resistor It!) and condenser I iI, both of which'aregrounded, serves to minimize or eliminate parasitic oscillations thatmight render the output less monochromatic. The resistor I42 providesgrid bias for the power amplifier tubes I43 and Mt. Transformer Hitprovides power for the filaments of the power tubes I43 and I'M, Thesetubes amplify power provided by circuit I22, imparting thereto thefrequency developed by oscillator tubes i152 and I33. connected with a1l0-volt supply, provides the energy to the power supply rectificationtubes Hi1 and hill. Transformer M9, also connected with a llIl-voltsupply, provides the power for the filaments of tubes It? and I48. Itwill be observed that circuit I22 is essentially similar to circuitiii]. The combination of the choke I50, fixed condenser I and resistorI52 constitutes a filter. The rectified power leaves the circuit viathemilliammeter I53 to ground and lead I li t to the power amplifiercircuit I2I. The voltage at which it is delivered is measured by thevoltmeter The power amplifier circuit I2I is tuned to the desiredfrequency is generated by means of oscillator tubes I32 and I 33 ofoscillator circuit I20 by means of the variable condenser I 56 and theinductance I51. The inductance I5! is varied by means of changing coilsto meet various wave length requirements as is done in the case ofinductances I36 and I38. The power amplifier circuit iti thus tuned andsupplied by D. C. power from circuit I22 transmits the amplified highfrequency energy to the coupling circuit I58, which in turn delivers itto a tank circuit such as is shown in Fig. 10.

Fig. represents a tank circuit of the type known as end grounded." Thecoupling cir- Transformer I46,

16 l I l I a that set forth in Fig. '2, the increase incapacity isapproximately in direct proportionto the increase in number of pairs ofelectrodes, it. being pointed out that each set of electrodes comprisesa primary hot electrode terminal and-acorresponding secondary or antennaelectrodetermicuit I 59, Fig. 10, is part of the same circuit I58 shownin Fig. 9. It is placed at the end of the inductance I60 instead of inthe middle, as would be the case if it were center grounded. The pointiIiI is the location of the hot electrode of the discharge, while 32, 33and 34 (Figs. 1 and 10) show the location of the antenna electrodes.Tuning of this tank circuit is accomplished by means of the variablecondenser I82 and by changing the inductance I60 to meet requirements.The circuit conductors I63 are preferably of copper tubing. The highfrequency voltmeter is shown at I64, and it will be noted that it has aground terminal I65 which is also the ground terminal for'the inductorI60. The hot electrode 9 of Fig. 1 and NH of Fig. 10 connect into thetank circuit by means of conductor 2| (Figs. 1 and 10). This tankcircuit was used in carrying out both of the examples hereinbefore setforth.

In employing reactors of the type herein set forth, the productioncapacity is greatly increased. When employing a reactor typified by nal.If the capacity of the reactor of, Fig. 7 is 3 grams per hour for eachset or pair of electrodes. then the total capacity of the reactor, asshown, is approximately 9 grams per hour. It is within the province ofthe present invention to provide a reactor of the type shown in Fig. 7,but wherein, instead of 3 pairs of primary and secondary electrodes,there are provided 100 pairs of primary and secondary electrodes, eachpair of said electrodes comprising a hot electrode and an antennaelectrode. Such a reactor will have a capacity per hour of 300 grams.

As pointed out, the basic discoveries herein set forth may beincorporated in a reactor employing the principle of crossed discharges.In connection therewith, it may be pointed out that if the reactor ofFig. 7 is operated with one pair of high frequency electrodes there willbe a given output per hour. If the electrodes of said reactor arecrossed with low frequency electrodes, as set forth in said copendingapplication Serial No. 546,882, filed July 27, 1944, Electrochemicaltransformation of gaseous material, a continuation in-part ofapplication Serial No. 483,931, now abandoned, and atmospheric air orequivalent material is electrically transformed to produce nitric acid,then thereresults an increase in chemical'yield of nitric acid perkilowatt hour which is greater than the sum of the yield perkilowatthour produced by passing air through a .reactor having highfrequency electrodes carrying the same high frequency; and the yield perkilowatt hour produced by passing air through a reactor having the samelow frequency energy passing through its electrodes as passed throughthe low frequency electrodes of the reactor provided with crossedelectrodes. This increase in chemical yield is characteristic of acrossed discharge reactor such .as set forth in Example I, andsimultaneously with this increase in chemical yield so ChflI'aC-teristic of crossed discharges, as particularly pointed out in saidcopending application, there is a tremendous increase in capacity, thisbeing due to the provision of a plurality of pairs of high frequencyelectrodes. I i

In the production of nitric oxide and, in general, in theelectrochemical transformation of materials, it is within the provinceofthe present invention to carry out the reaction undera vacuum, or atatmospheric pressure, 'or 'at superatmospheric pressure.

The present invention, while specifically adapted for the production ofnitric oxide, may beused for the electrochemical transformation of manydifferent chemical entities. Nitric oxide maybe produced by passingthrough the reactora nitrogen and oxygen-containing medium in which thenitrogen and oxygen gases are'present in various proportions, andincludes air,whichis a. naturally-occurring mixture of oxygen andnitrogen gases, or a synthetic mixture containing nitrogen gas andoxygen gas. Eachof saidmixtures may have present a diluent gas,' s omeof which assists in promotingthe reaction' so'l as to produce nitrogenoxides, as, for example, "nitric oxide, said diluent gas preferablybeing an inert gas, as, for example, helium, neon, andithe like.

The present invention provides for increased production capacity of thereactor, increased chemical yield per e hour n er life oi as isle lrqset sm a ianda upi pejireact rl m:

mine th th prse w e fb P Qfld d-Wii anten a g. of .th efreactor oppositethe h e leg toprovidea 'compact and eflicient',reactor, the capacity, of.whi ch is much g eat r, them afslnillar crossed discharge reactorwhichlisiiot provided with a'plurality of antenna I L e method andapparatus for increasctrical transfer andchemical efliciency ioicapacity by' employing split disan e na t o s i the nve tion sewera e; rm 30- if -ito1?a0 i an more, usually a frequency,from fiomc;.to3,000

meansto remove transformed material from said reactor; chamber;agprimary high-potential ;elec trode. inazsaidachamber connected 1 to:said .source of; -.'cyclic,,-.'energy, said electrode ,1 being providedwith :aplurality ofelectrode terminalsrdistribut- I Dento' iandisbroadlycl'aime'dinappli the electrochemicalt of gage ous materia1, thecombination of a source or cyclic energy iha vi ng a frequency of atleast 300,000'cyc1es, and a reactor'comprising a reactor chamber, asheath member therein, means con-- nected, to said sheath member tointroduce reacting material into the reactor chamber, a prif ry high"potential electrode mounted in said shathfmemb and connected to saidsource of cyclic energyf-s'a'id electrode, being provided with aplurality of electrode terminals distributing cyclic energy subplicdtosaid electrode to thereby increase the' lworking lifeoi theriaactorand simultaneously increase the chemical efliciency bifthereactor' 'a s'econd sheath member mounte'd'jin saidlreactor chamber,means connectedto saidfsheath'finember forremoving reaction pro-'- d'icts from; the reactor chamber, a plurality of sCDndary electrodesmounted in said second sheath member,feach of said electrodes beingprovi d with, a secondary electrode terminal, said assemblagegprovidinga plurality of pairs of electrbdeterminals, an antenna member separatelyconnected to each of said secondary cooperating electrodes, and means totune each antenna each of the latter being in circuit with. said sourceof cyclic electrical energy to thereby insure transfer of electricalenergy from the source of said energy to the reactor with relatively lowtransfer loss.

3. The method of effecting the electrochemical transformation of agaseous material in a reactor comprisinga'reactor chamber, a highpotential electrode therein provided with a plurality of high potentialelectrode terminals and a plurality of ,cooperatinglow potentialelectrodes and electrode terminals, said low potential units beingseparatelyspacedfrom each other and electrically independent ofeachother, said assemblage of @lctrodes and terminals being adapted to haveluminous electrical'disch'arges pass therebetween, comprisingefiec'ting. said transformationin the presence of 1a luminous dischargeand with little heat decomposition of the transformed product whileprolongin the working life of the electrode terminals byv supplying tosaid high potential electrodehi'ghfr'equencyenergy having a frequency mgcyclic-welectrical;energy; supplied-g to said elec'- trodeito vthereby;increase the working life 1 erthe reactor;andisimultaneouslyeincreasethe chemical efliciency f'ofztheireactor, -a-= plurality?- of secondaryelectrodes 11in .s'aidllreactor chamber, :eachi thereof being providedwith a secondary electrode .term'ie 1 l of over 300,000cycle's,distributing the cyclic energy supplied to said high potential electrodetosaid high potential electrode terminals and passing the so-distributedenergy to a plurality of separately spaced lowpotential electrodes andlow potential electrode terminal units, each unit being electricallyindependent of each other unit, and separately tuning eachof said.independent low potential electrodeunits.

I 4. In an electrochemical apparatus for efifecting the electrochemicaltransformation of gaseous material. in the presence of a luminous cyclicelectrical discharge, the combination of a source of lcyclicflenergy,"comprising a reactor chamber, meansto therein introduce reactingmaterial,

' means tofremove reaction products from said of cyclic electricalenergy to thereby insuretrans (fer- OfF eIectricaI 5 energy irom thesource or. said energymoihenreactor with relat'ivlelyi-lo transfer loss;audan'eansrtotune each antenna 5! i2..In' ntelectrochemica an ar his tofiecte chamber, a primary high potential electrode ,in said reactorchamber connected to said source ofjc'yclic'energy, saldfelectrode beingprovided with a plurality of electrode terminals distribut ingcyclicelectrical energy supplied to said electrode to thereby increasetheworking life of the reactorga-plurality of secondarylow potentialelectrodes in said reactor chamber, each electrode thereofbeinglprovided with a secondary low potential electrode terminal, saidassemblage prorld sa p u al t io a r'sfl le t e m nals ac io iseies enda ceqe a 'sh-f ing;-,separately connected to a separate antenna.

including tuning means in circuit with said source of cyclic electricalenergy to thereby insure trans ter of electrical energy from the sourceof said energy to the reactor with relatively low transfer loss, andmeans for producing a cyclic electrical discharge crossing the luminouscyclic discharge generated by the primary high potential electrodeterminals and secondary low potential electrode terminals.

5. In a gas discharge apparatus for 'eflecting the electrochemicaltransformation of gaseous material in the presence of a luminous cyclicelectrical discharge, the combination of an electrical circuitfurnishing cyclic electrical energy,

a reactor chamber, means for introducing gase ous material therein,means for removing transformed material therefrom, a primary high po-'tential electrode in said reactor chamber con nected in said electricalcircuit and receiving cyclic energy and having a plurality of electrodeterminals spaced from each other whereby the electrical energy suppliedto the high potential primary electrode is distributed to said electrodeterminals, a plurality of tuneable low potential cooperating secondaryelectrodes and electrode terminal units in said reactor chamberseparately spaced from each other and from the high potential primaryelectrode terminals, each of said low potential units being electricallyindependent of each other, and means including means to tune said lowpotential electrode units to cause luminous discharges to be initiatedand maintained between said high potential primary electrode terminalsand the secondary low potential electrode terminals.

6. In a gas discharge apparatus for effecting the electrochemicaltransformation of gaseous material in the presence of a luminous cyclicelectrical discharge, the combination of an electrical circuitfurnishing cyclic electrical energy, a reactor chamber, means forintroducing gaseous material therein, means for removing transformedmaterial therefrom, a primary high potential electrode in said reactorchamber connected in said electrical circuit and receiving cyclic energyand having a plurality of electrode terminals spaced from each otherwhereby the electrical energy supplied to the high potential primaryelectrode is distributed to said electrode terminals, a plurality of lowpotential cooperating secondary electrode terminals in said reactorchamber separately spaced from each other and from the high potentialprimary electrode terminals, an antenna connected to each of saidseparately spaced low potential electrodes, the latter and each antennabeing in circuit with the source of cyclic electrical energy, and meansto tune each antenna and thereby cause luminous electrical discharge tobe initiated and maintained between said high potential primaryelectrode terminals and the secondary low potential elec-' trodeterminals.

7. In a gas discharge apparatus for effecting the electrochemicaltransformation of gaseous material in the presence of a luminous cyclicelectrical discharge, the combination of a generator unit furnishingcyclic electrical energy, said generator unit being coupled to a tankcircuit containing a reactor having a reactor chamber, means forintroducing gaseous material therein, means for removing transformedmaterial therefrom, a primary high potential electrode in said reactorcyzlmmbcr connected in said electrical circult and receiving cyclicenergy and having a plurality oi electrode terminals spaced from each 201 other whereby the electrical energy supplied the high potentialprimary electrodeisdistributed to said electrode terminals, apluralityjoii tuneable low potential cooperating secondary electrode andelectrode terminal separately spaced from each other and from the highpotential primary electrode terminals, each of said low potentialunitsbeing electrically in-- dependent of each other, means in the tankcircult to eflect tuning of said low potential electrode units and causeluminous discharges to be initiated and maintained between said highpotential primary electrode terminals and the secondary low potentialelectrode terminals.

8. In a gas discharge apparatus for effecting the electrochemicaltransformation of gaseous material in the presence of a luminous cyclicelectrical discharge, the combination, of a' generator unit furnishingcyclic electrical energy, said generator unit being, coupled to a. tankcircuit containing a reactor having a reactor chamber. means forintroducing gaseous material therein, means for removing transformedmaterial there from. a primary high potential electrode in said reactorchamberconnected in said electrical circuit and receiving cyclic energyand having a plurality of electrode other whereby the electricalenergyisupplied to the high potential primary to said electrodeterminals, a pluralityof low potentlal cooperating secondary electrode"terminals m said reactor chamber separately spaced from ,each other andfrom the electrode terminals, an antenna connected to each of saidseparately spaced low potential electrodes. the latter, the antennaeandthelligh potential electrode terminals being part of the tankcircuit,

and means to tune each antenna and thereby cause luminous electricaldischarges to be initiated and maintained between said high potentialprimary electrode terminals and low potential secondary electrodeterminals.

9. In a gas discharge apparatus for efl'ecting the electrochemicaltransformation or gaseous material in the presence of a luminouscyclicelectrical discharge, the combination of an electrical circuitfurnishing cyclic electrical energy,

a reactor chamber, means for introducing gaseous material therein, meansfor removing transformed material-therefrom, a primary high potentialelectrode in said reactor chamber-connected in said electrical circuitand receivlng cyclic energy and having a plurality of electrodeterminals spaced from each other whereby the electrical energy suppliedto the high potential primary electrode is distribtuedin said electrodeterminals, a plurality of low potential cooperating secondary electrodeterminals in said reactor chamber separately spaced from eachother andfrom the high potential primary electrode terminals, means includingmeans to tune said electrical circuit to cause luminous discharges to beinitiated and maintained between said 'high potential primary electrodeterminals andathesecondary low potential electrode terminals, and meansfor producing a cyclic electricaldischarge crossing the luminous cyclicelectrical "discharge generated by the high potential primary, electrodeterminals and the secondary low potential electrode terminals.

10. In a gas discharge apparatus for effecting the electrochemicaltransformation oi gaseous material in the presence 01. a luminous cyclicelectrical discharge, the combination of an electrical circuitfurnishing cycliw'clectrlcal energy, a reunits in said reactor chamberterminals spacedj from each electrodeis'distrlbuted high potentialPrimary mean's' for introducing gaseous e. a 'i s r H ntia el trodeflnsaid"reactor-chambercon id electrical circuit and -reeelvingacdf-fronr'each other seconda y electrode,terminalsu in, said reactorchamber separately spac'ed' frdm 'ach other and I ironn heehishrmtetialmrima r ectro eate minals, an antenna connecte each oi; saidseparately;,spaced low.,p lifintia el trodes, the latter and each'antenna" being sourclerfl cyclic electrical energy, meansitostunetrical'adischargesto be vinitiated :and maintained betweemssaid highpotential -priniary=; electrode aterminals and,theisecondaryr wii tntiali le itrode terminals,,and,meansior producingi a": cyclicelectricaiadischarge. crossing;,-the,, uminquswyclicielecti'lcaladischarge generated bygthe high potenarylom ndten a ififictrcde ter ina itorunitafnrnishing cyclic energy: of a irequency of atleastl0,000 cyclesper se,cond, ,said generator unit being coupledto'a'tank circuit containing a reactor having a reactor; chamber, means;for

introducin'g gaseous, material-;.therein, means for removingtransformed. material, therefrom, a 5; primary highpotentia1e1ectrcde*-in said reactorfichambeinconnectemintsaidielectrical circuitrfand receivingcyclicienergyz-iand ihavingiiai gpluralit'y of electrode terminalsspaced from each other whereby the electrical energy supplied to thehigh potential primary electrode is distributed to said electrodeterminals, a plurality of low potential cooperating secondary electrodeterminals in said reactor chamber separately spaced from each other andfrom the high potential primary electrode terminals, means in the tankcircuit to efiect tuning and cause luminous discharges to be initiatedand maintained between said high potential primary electrode terminalsand the secondary low potential electrode terminals, and means forproducing a cyclic electrical discharge crossing the luminous cyclicelec trical discharge generated by the high potential primary electrodeterminals and the secondary low potential electrode terminals.

12. In a gas discharge apparatus for effecting the electrochemicaltransformation of gaseous material in the presence of a luminous cyclicelectrical discharge, the combination of a generator unit furnishingcyclic energy or a frequency of at least 10,000 cycles per second, saidgenerator unit being coupled to a tank circuit containing areactorhaving a reactor chamber, means for introducing gaseousmaterialtherein, means for removing transformed material therefrom, aprimary high. potential electrode in said reactor chamber connected insaid electrical circuit and receiving cyclic energy and having aplurality of electrode terminals spaced from each whereby the electricalenergy supplied to the high potential primary electrode is distributedto said electrode terminals, a plurality of low potential I cooperatingsecondary electrode terminals in said reactor chamber separately spacedfrom each nd havin'g a plurality of electrode 1 can with theeachgantepna and thereby; ,causej- ;luminous ,relecitallprimaraaielectrod te in l a h econ other and from the high potentialprimary elec-- trode terminalsan-antenna connected to each of saidseparately 'spaced-low'potenti'al electrodes,

the" latter, the antennae and the high potential 5 electrode terminalsbeing part of the tank circuit, means totune 'each a'ntenna and therebycause luminous-electrical discharges to be initiatedand maintainedbetween said high potential primary electrodeterminals and thelowpotential secorida'ry' electrod terminalsand met as for produping acycIi'c electrical discharge crossing-the luminous "cyclicel'ect'ric'aldischarge generated by t high 'pbtntial primary electrode terminals 'a dthe-secondary low potential electrode ter 3; The" "ethod or effectingthe electrochemibfen' a high-' pote'ntial"primary electrode thereinprovided Wlth-a-plurality of primary electrode terminals anda'pluralityor separately spaced 'tuneable'cooprating low potential secondaryelectrode and electrode terminal units therein, said low potentialelectrode and electrode termi- 'ri'alunits' 5 being-"electricallyindependent of one another;'said'fasseniblageof electrodes and terminalsbeingadapted to have a luminous electrical discharge pass from eachprimary high pcltential electrode terminal to its cooperating sec-"o'ndarylow potential electrode terminal comprising'effecting'saidtransformation with little heat decomposition of the transformed productby supplying cyclicelectrical energy to said high potential electrode;distributing said energy to said plural'ity of high 'poten'tialelectrode terminals, and passing*the so supplied energ'y'to a plurality'of arately spaced low potential electrode and f'lo-polx'nitiaP'ele'cztrode terminal units, each unit being electricallyindependent of each other and separately tuning each of said independentlow potential electrode units.

14. The method of effecting the electrochemical transformation of agaseous material in a gas discharge reactor constituting a portion oi aplurality of electric circuits, said reactor comprismg a reactorchamber, a high potential primary electrode therein provided with aplurality of primary electrode terminals and a plurality of separatelyspaced tuneable cooperating low potential secondary' electrode andelectrode termi nal units therein, said low potential electrode andelectrode terminal units bein electrically independent of one another,said assemblage of electrodes and terminals being adapted to have aluminous electrical discharge pass from each primary high potentialelectrode terminal to its cooperating secondary low potential electrodeterminal, comprising eflecting said transformation in the presence of aluminous discharge with little beat decomposition of the transformedproduct while prolonging the working life of the electrode terminals bysupplying to said high potential electrode electrical energy having afrequency of at least 10,000 cycles per second, pass- 65' ing theso-supplied energy to a plurality of low potential electrode and lowpotential terminal units, each of said units being electrically inde- Pndent of each other, and tunin the electrical circuits to'initiate andmaintain luminous electrical discharges between said primary highpotential electrode terminals and their low potential cooperatingelectrode terminals,

15. In a gas discharge apparatus for effecting the electrochemicaltransformation of gaseous material in the presence of a luminous cycliceleov calf-transformation of -a' gaseous material in a gasgais'chargereactor comprising a reactor chainearn trical discharge, the coinatlonof a generator unit furnishing cyclic energy'of a frequency o!" at least10,000 cycles per second, said generator unit being coupled to a tankcircuit containing a reactor having a reactor chamber, means forintroducing gaseous material therein, means for removingtransformedmaterial therefrom, a pri mary high potential 'electrode'insaid reactor in seid reacto'r chamber separatelyfshacedirom to saidelectrode terminals, apluralit'yl-o'tlompotential cooperatingsecondaryelem-mammal each other and i'rom the high potential primary electrodeterminals, and, means ,ior tuningl each of the discharges between s'a'idelectrode, terchamber connected in said electrical circuit and electrodeterminals, 9; plurality of low potential cooperating secondary electrodeterminals in said reactor chamber separately spaced from each 7 otherand'from the high potential, primary elec trode terminals, and means inthe tank circuit to effect tuning and cause luminous discharges to beinitiatedand maintained'between saidhigh potential primary electrodeterminals and the secondary low, potential electrode terminals.

16.,In a gas dlschargeiapparatusfor effecting 'the electrochemicaltransformation of gaseous material in. the presence 01a luminous cyclicelectrical discharge. the combination or a generator unit furnishingcyclic energy of aIfre quency of at least 10,000 cycles per second, saidgenerator unit being coupled to a tank circuit containing a reactorhaving a reactorchamber', means for introducinggaseous material therein,

7 meansfor removing transformed material therefrom. a primary'highpotential electrode in said reactor chamber connected in said electricalcircuit and receivingcyclio energy and having a plurality of electrodeterminals spaced from each other whereby the electrical energy suppliedto the high potential primary electrode is distributed minals within thetank energy transfer efilciency. i 1 1 l J, COTEON. nnrannncns Thefollowing references are of record in the file of this patentzf w t i IsnsTA'rEsr-ATEnc-s Number Name Date- 1 546,702 wxonemaniuu Sent'. :24,1895 659,926 Jacobs' ",...*Oct.26; 1900 a 908,291 Martini Dec29p19081,055,331 Kochmann '11; 1913' 1,290,471 Hcofnagle woes 1,1915 1,376,180wickershamuer ADL'QB, 1921 1,615,645 Nyman 3911425, '192? 1,673,654 WeedJune12,1928 1,912,499 Jakosky et al. flan. 29,1935 7 1,999,499 sabotr.,-Jan; 29,1935 2,043,422 Bergk et 9.]. James, 1938 2,064,260 Dec, 15, 193B7 2,090,930 I i I .,-May 1a, 1937 2,106,780 A Whittier *Feb: :1."199s Iseamen m'rsn'rs 1 Number @.-Co'untry 67,583 Switzerland Dec; 3. 1913'circuit tot-increase the (recreate cc

